Xu Tang,Wenjing Shen,Dongyi Li,Binrong Li,Yemei Wang,Xianghai Song,Zhi Zhu,Pengwei Huo
The novel Co-doping combined with mesoporous g-C 3 N 4 -based photocatalyst was constructed, and the Co-CN showed impressive photocatalytic reduction CO 2 activity. Employing the DFT computation, we discussed the possible Co doping sites on g-C 3 N 4 framework, as well as the effects of band gaps, optical properties , and various densities of state (DOS) on photocatalytic activity. The adsorption energy calculation proved that the substitution and interstitial doping Co atoms in g-C 3 N 4 crystal unit cell was the stable configuration. The coexistence substitution and substitution the monolayer g-C 3 N 4 showed serious deformation. It indicated that the introduction of Co atoms leads g-C 3 N 4 molecular orbital redistribution and Co tends to occupy the conduction band, due to its weak electronegativity. Moreover, the DFT and experiment results pointed out that the doped-Co narrowed g-C 3 N 4 bandgap and increased light absorption from 450 to 800 nm, the improved charge carrier separation efficiency was originated from Co atom the unfilled 4 f and the empty 5d orbital act as electron capturing center. This research indicates the availability of transition metal g-C 3 N 4 with conducive photocatalytic activity.
Graphical Synopsis: A pyrrolic N-rich g-C 3 N 4 (PN-g-C 3 N 4 ) framework is synthesized with transition metal M (M=Fe, Co, Ni, Cu, Cr, and Mn) atomic sites coordinated onto it. M/PN-g-C 3 N 4 are constructed for peroxodisulfate activation. The synergy between photocatalysis and Fe/PN-g-C 3 N 4 catalyst results in increased generation and separation of charge carriers, along with the cyclic transformation of the Fe 3+ /Fe 2+ couple. Photocatalysis is an efficient technology for the degradation of pollutants. However, there is still much room for improvement in its degradation efficiency. In this study, a pyrrolic N-rich g-C 3 N 4 (PN-g-C 3 N 4 ) framework was synthesized with transition metal M (M=Fe, Co, Ni, Cu, Cr, and Mn) atomic sites coordinated onto it. Then, a series of single atomic metals M anchored to PN-g-C 3 N 4 (M/PN-g-C 3 N 4 ) are constructed for peroxodisulfate activation. Their order of catalytic activity follows Fe>Cr>Ni>Cu≈Co>Mn, in particular the degradation rates of the TCH for Fe-PN-g-C 3 N 4 are 3.74 times higher than that of undoped PN-g-C 3 N 4 . These carefully regulated pyrrolic N-rich Fe sites demonstrate outstanding performance in degrading organic pollutant. As an exemplary model, the Fe/PN-g-C 3 N 4 catalyst efficiently drives the catalytic oxidation of TCH through Fenton-like reaction under visible light, showcasing exceptional cycle stability and a broad effective pH range of 3.0–11.0. The synergy between photocatalysis and Fe doped catalysis results in increased generation and separation of charge carriers, along with the cyclic transformation of the Fe 3+ /Fe 2+ couple. This combination significantly enhances the Fenton-like performance, making it a highly effective process for pollutant degradation.
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